A theoretical study of the reverse water-gas shift reaction on Ni(111) and Ni(311) surfaces

Min Zhang, Bart Zijlstra, Ivo Filot, Fang Li, Haiou Wang, Jingde Li (Corresponding author), Emiel Hensen (Corresponding author)

Onderzoeksoutput: Bijdrage aan tijdschriftTijdschriftartikelAcademicpeer review

Uittreksel

This paper presents a systematic comparison study of the surface redox reaction mechanism for reverse water-gas shift (RWGS) over Ni(111) and Ni(311) surfaces. Specifically, the most stable surface intermediates and the reaction kinetics involved in the direct CO 2 activation and water formation steps are computed with density functional theory calculations and compared for the two different Ni surfaces. The results show that CO 2, CO, O, H, OH, and H 2O species adsorb stronger on Ni(311) than on Ni(111). Compared to Ni(111), the overall barriers for direct CO 2 activation and water formation on Ni(311) are lower by 23 and 17 kJ/mol, respectively. These observations indicate that the RWGS reaction through the surface redox mechanism should be preferred on Ni(311).

Originele taal-2Engels
Pagina's (van-tot)740-748
Aantal pagina's9
TijdschriftCanadian Journal of Chemical Engineering
Volume98
Nummer van het tijdschrift3
DOI's
StatusGepubliceerd - 1 mrt 2020

Vingerafdruk

Water gas shift
Carbon Monoxide
Chemical activation
Water
Redox reactions
Reaction kinetics
Density functional theory

Citeer dit

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title = "A theoretical study of the reverse water-gas shift reaction on Ni(111) and Ni(311) surfaces",
abstract = "This paper presents a systematic comparison study of the surface redox reaction mechanism for reverse water-gas shift (RWGS) over Ni(111) and Ni(311) surfaces. Specifically, the most stable surface intermediates and the reaction kinetics involved in the direct CO 2 activation and water formation steps are computed with density functional theory calculations and compared for the two different Ni surfaces. The results show that CO 2, CO, O, H, OH, and H 2O species adsorb stronger on Ni(311) than on Ni(111). Compared to Ni(111), the overall barriers for direct CO 2 activation and water formation on Ni(311) are lower by 23 and 17 kJ/mol, respectively. These observations indicate that the RWGS reaction through the surface redox mechanism should be preferred on Ni(311).",
keywords = "DFT, carbon dioxide, nickel, reverse water-gas shift, surface redox",
author = "Min Zhang and Bart Zijlstra and Ivo Filot and Fang Li and Haiou Wang and Jingde Li and Emiel Hensen",
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month = "3",
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doi = "10.1002/cjce.23655",
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A theoretical study of the reverse water-gas shift reaction on Ni(111) and Ni(311) surfaces. / Zhang, Min; Zijlstra, Bart; Filot, Ivo; Li, Fang; Wang, Haiou; Li, Jingde (Corresponding author); Hensen, Emiel (Corresponding author).

In: Canadian Journal of Chemical Engineering, Vol. 98, Nr. 3, 01.03.2020, blz. 740-748.

Onderzoeksoutput: Bijdrage aan tijdschriftTijdschriftartikelAcademicpeer review

TY - JOUR

T1 - A theoretical study of the reverse water-gas shift reaction on Ni(111) and Ni(311) surfaces

AU - Zhang, Min

AU - Zijlstra, Bart

AU - Filot, Ivo

AU - Li, Fang

AU - Wang, Haiou

AU - Li, Jingde

AU - Hensen, Emiel

PY - 2020/3/1

Y1 - 2020/3/1

N2 - This paper presents a systematic comparison study of the surface redox reaction mechanism for reverse water-gas shift (RWGS) over Ni(111) and Ni(311) surfaces. Specifically, the most stable surface intermediates and the reaction kinetics involved in the direct CO 2 activation and water formation steps are computed with density functional theory calculations and compared for the two different Ni surfaces. The results show that CO 2, CO, O, H, OH, and H 2O species adsorb stronger on Ni(311) than on Ni(111). Compared to Ni(111), the overall barriers for direct CO 2 activation and water formation on Ni(311) are lower by 23 and 17 kJ/mol, respectively. These observations indicate that the RWGS reaction through the surface redox mechanism should be preferred on Ni(311).

AB - This paper presents a systematic comparison study of the surface redox reaction mechanism for reverse water-gas shift (RWGS) over Ni(111) and Ni(311) surfaces. Specifically, the most stable surface intermediates and the reaction kinetics involved in the direct CO 2 activation and water formation steps are computed with density functional theory calculations and compared for the two different Ni surfaces. The results show that CO 2, CO, O, H, OH, and H 2O species adsorb stronger on Ni(311) than on Ni(111). Compared to Ni(111), the overall barriers for direct CO 2 activation and water formation on Ni(311) are lower by 23 and 17 kJ/mol, respectively. These observations indicate that the RWGS reaction through the surface redox mechanism should be preferred on Ni(311).

KW - DFT

KW - carbon dioxide

KW - nickel

KW - reverse water-gas shift

KW - surface redox

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